We present a facile route to deposit a uniform Al2O3 layer on a highly oriented pyrolytic graphite (HOPG) surface using atomic layer deposition (ALD). Al2O3 layers deposited from TMA (trimethylaluminum)/ H2O chemistry showed selective deposition only on step edges. However, TMA/O3 chemistry resulted in the deposition of Al2O3 layers on basal planes of HOPG, which has a chemically inert surface. An O3-pretreatement followed by Al2O3 deposition using TMA/O3 chemistry produced conformal and uniform Al2O3 dielectric layers with a small RMS roughness of ~ 0.2 nm. This suggests that O3-pretreatement prior to ALD deposition makes the chemically inert HOPG surface reactive toward ALD precursors, which leads to the desired two-dimensional growth mode. High-resolution transmission electron microscopy (HR-TEM) and Raman spectroscopy revealed that this O3 process used for Al2O3 deposition does not introduce a significant defect concentration to the top graphene layer. The dielectric constant of the deposited Al2O3 film on top of the HOPG surface was found to be ~ 9 from C-V measurements.
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